Second-Harmonic Generation-Positive Na2Ga2SiS6 with a Broad Band Gap and a High Laser Damage Threshold
The development of high-power solid-state lasers is in urgent need of new infrared nonlinear optical (IR NLO) materials with a wide band gap and a high laser-induced damage threshold. A new infrared nonlinear optical material Na2Ga2SiS6 has been synthesized for the first time, crystallizing in the Fdd2 (no. 43) noncentrosymmetric space group. Its three-dimensional tunnel framework consists of two typical NLO active motifs [GaS4] and [SiS4], with Na+ cations located inside the tunnels. Na2Ga2SiS6 exhibits comprehensive optical properties, namely, a wide transmission range, a high laser-induced damage threshold (10 × AgGaS2), a type-I phase-matching second-harmonic generation response (0.2 × AgGaS2), and especially a wide band gap (3.93 eV), which is the largest in the A2MIII2MIVQ6 (A = alkali metals; MIII = IIIA elements; MIV = IVA elements; Q = S and Se) family. Therefore, Na2Ga2SiS6 does not produce two-photon absorption under a 1064 nm laser pump and could be used in high-energy laser systems, which makes Na2Ga2SiS6 a promising candidate for high-energy IR NLO applications.
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